Tailoring the Electronic Structure and Properties of Graphdiyne by Cyano Groups

Two-dimensional (2D) materials, such as 2D carbon-based systems, have been recently the subject of intense studies, thanks to their optoelectronic properties and promising electronic performances. 2D carbon-based materials such as graphdiyne (GDY) represent an optimal platform for tuning the optoele...

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Published inACS nano Vol. 18; no. 44; pp. 30368 - 30377
Main Authors Gao, Lei, Wang, Shuailong, Wang, Fan, Yang, Ze, Li, Xiaodong, Gao, Jingchi, Fazzi, Daniele, Ye, Xiang, Wang, Xuebin, Huang, Changshui
Format Journal Article
LanguageEnglish
Published United States American Chemical Society 05.11.2024
Subjects
graphdiyne
energy gap regulation
functional group editing
lithium-ion battery
cyano groups
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Abstract Two-dimensional (2D) materials, such as 2D carbon-based systems, have been recently the subject of intense studies, thanks to their optoelectronic properties and promising electronic performances. 2D carbon-based materials such as graphdiyne (GDY) represent an optimal platform for tuning the optoelectronic properties via precise chemical functionalization. Here, we report a synthetic strategy to precisely introduce cyano groups into the 2D GDY backbone in order to tune the electronic properties of GDY. Three kinds of cyano-modified GDY have been synthesized, namely, bearing one cyano group (CNGDY), two CN in meta (m-CNGDY), and two in para (p-CNGDY) positions. A variety of experimental data as well as first-principles calculations allowed us to elucidate the role of the cyano groups in tuning the structural and functional properties of GDYs. We found that an increase in the number of cyano groups reduces the interlayer spacing between GDY layers, increases the lithium adsorption amount, as well as impacts the lithium diffusion rate, while changes in meta- or para-position impact the energy band gap.
AbstractList Two-dimensional (2D) materials, such as 2D carbon-based systems, have been recently the subject of intense studies, thanks to their optoelectronic properties and promising electronic performances. 2D carbon-based materials such as graphdiyne (GDY) represent an optimal platform for tuning the optoelectronic properties via precise chemical functionalization. Here, we report a synthetic strategy to precisely introduce cyano groups into the 2D GDY backbone in order to tune the electronic properties of GDY. Three kinds of cyano-modified GDY have been synthesized, namely, bearing one cyano group (CNGDY), two CN in meta (m-CNGDY), and two in para (p-CNGDY) positions. A variety of experimental data as well as first-principles calculations allowed us to elucidate the role of the cyano groups in tuning the structural and functional properties of GDYs. We found that an increase in the number of cyano groups reduces the interlayer spacing between GDY layers, increases the lithium adsorption amount, as well as impacts the lithium diffusion rate, while changes in meta- or para-position impact the energy band gap.
Two-dimensional (2D) materials, such as 2D carbon-based systems, have been recently the subject of intense studies, thanks to their optoelectronic properties and promising electronic performances. 2D carbon-based materials such as graphdiyne (GDY) represent an optimal platform for tuning the optoelectronic properties via precise chemical functionalization. Here, we report a synthetic strategy to precisely introduce cyano groups into the 2D GDY backbone in order to tune the electronic properties of GDY. Three kinds of cyano-modified GDY have been synthesized, namely, bearing one cyano group (CNGDY), two CN in meta ( -CNGDY), and two in para ( -CNGDY) positions. A variety of experimental data as well as first-principles calculations allowed us to elucidate the role of the cyano groups in tuning the structural and functional properties of GDYs. We found that an increase in the number of cyano groups reduces the interlayer spacing between GDY layers, increases the lithium adsorption amount, as well as impacts the lithium diffusion rate, while changes in meta- or para-position impact the energy band gap.
Two-dimensional (2D) materials, such as 2D carbon-based systems, have been recently the subject of intense studies, thanks to their optoelectronic properties and promising electronic performances. 2D carbon-based materials such as graphdiyne (GDY) represent an optimal platform for tuning the optoelectronic properties via precise chemical functionalization. Here, we report a synthetic strategy to precisely introduce cyano groups into the 2D GDY backbone in order to tune the electronic properties of GDY. Three kinds of cyano-modified GDY have been synthesized, namely, bearing one cyano group (CNGDY), two CN in meta (m-CNGDY), and two in para (p-CNGDY) positions. A variety of experimental data as well as first-principles calculations allowed us to elucidate the role of the cyano groups in tuning the structural and functional properties of GDYs. We found that an increase in the number of cyano groups reduces the interlayer spacing between GDY layers, increases the lithium adsorption amount, as well as impacts the lithium diffusion rate, while changes in meta- or para-position impact the energy band gap.Two-dimensional (2D) materials, such as 2D carbon-based systems, have been recently the subject of intense studies, thanks to their optoelectronic properties and promising electronic performances. 2D carbon-based materials such as graphdiyne (GDY) represent an optimal platform for tuning the optoelectronic properties via precise chemical functionalization. Here, we report a synthetic strategy to precisely introduce cyano groups into the 2D GDY backbone in order to tune the electronic properties of GDY. Three kinds of cyano-modified GDY have been synthesized, namely, bearing one cyano group (CNGDY), two CN in meta (m-CNGDY), and two in para (p-CNGDY) positions. A variety of experimental data as well as first-principles calculations allowed us to elucidate the role of the cyano groups in tuning the structural and functional properties of GDYs. We found that an increase in the number of cyano groups reduces the interlayer spacing between GDY layers, increases the lithium adsorption amount, as well as impacts the lithium diffusion rate, while changes in meta- or para-position impact the energy band gap.
Author Fazzi, Daniele
Gao, Lei
Wang, Xuebin
Gao, Jingchi
Yang, Ze
Li, Xiaodong
Wang, Shuailong
Wang, Fan
Huang, Changshui
Ye, Xiang
AuthorAffiliation Shandong University of Science and Technology
Science Center for Material Creation and Energy Conversion, Institute of Frontier and Interdisciplinary Science
College of Energy Storage Technology
Department of Chemistry “Giacomo Ciamician
National Laboratory of Solid-State Microstructures (NLSSM), Collaborative Innovation Center of Advanced Microstructures, Jiangsu Key Laboratory of Artificial Functional Materials, College of Engineering and Applied Sciences
Beijing National Laboratory for Molecular Sciences, Organic Solids Laboratory
Department of Physics
University of Chinese Academy of Sciences
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energy gap regulation
functional group editing
lithium-ion battery
cyano groups
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Title Tailoring the Electronic Structure and Properties of Graphdiyne by Cyano Groups
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